Organic　electrode　materials　are　potential　energy　storage　materials　for　the　next　generation　lithium　batteries.　Herein,　carboxylate　groups　are　installed　to　a　conjugated　tetrathiafulvalene　(TTF)　platform　to　yield　two　compounds,　namely　lithium　tetrathiafulvalene-dicarboxylate　(TTF-Li2)　and　lithium　tetrathiafulvalene-tetracarboxylate　(TTF-Li4),　as　stable　anode　materials　for　lithium　batteries.　The　low　solubility　in　the　electrolyte,　brought　about　by　the　carboxylate　groups,　and　high　rechargeability　ensured　by　the　conjugated　TTF　platform　lead　to　excellent　battery　performance.　After　cycling　at　a　current　density　of　0.5　C　for　120　cycles,　a　net　specific　capacity　of　108.19　mAh　g−1　and　217.55　mAh　g−1　is　obtained　for　the　TTF-Li2　and　TTF-Li4　anodes　containing　70　wt.%　of　active　materials,　corresponding　to　61.4　%　and　82.0　%　of　their　theoretical　capacities,　respectively.　The　density　functional　theory　(DFT)　calculation　confirms　the　well-delocalized　charge　for　both　TTF-Li2　and　TTF-Li4.　Therefore,　the　TTF-Li2　and　TTF-Li4　are　promising　anode　materials　for　lithium　batteries.　©　2022　Wiley-VCH　GmbH.